Hydrophobic Interface Engineering for Highly Reversible and Stable Zn Anodes

Rechargeable aqueous zinc batteries (AZIBs) with merits of high safety and high theoretical capacity are regarded as next‐generation energy storage devices. However, their practical application is hindered by the instable Zn anodes associated with the dendrite growth, parasite corrosion and side reactions. Developing a stable solid electrolyte interface is crucial for improving the cycling stability of Zn anodes. Herein, a hydrophobic interface is constructed on Zn anode through a simple heptafluorobutyrate acid etching route. The hydrophobic interface containing organic C─F, O─C═O and inorganic Zn─F bonds effectively address the issues of dendrites growth and parasitic reactions. Consequently, symmetric cells with acid‐treated Zn‐HA anodes achieve a prolonged lifespan of over 2000 h at 4.0 mA cm−2 and 1100 h at 10.0 mA cm−2. When paired with MnO2 cathode, the full cells deliver lower overpotential and outstanding cycling stability. This strategy provides a simple and feasible method to construct stable Zn anode for achieving high performance AZIBs. A hydrophobic interface containing organic C─F, O─C═O and inorganic Zn─F bonds is in situ constructed on Zn anode by the simple treatment in heptafluorobutyrate acid etching. The organic–inorganic hybrid interface increases the Zn‐ion flux, inducing uniform Zn deposition. Low overpotential, prolonged lifespan, and outstanding cycling stability are achieved for the AZIBs.